Organic electroluminescent apparatus and method of fabricating the same

ABSTRACT

In an organic electroluminescent apparatus according to the present invention, in arranging organic electroluminescent devices each having an organic layer having luminescent properties provided between a first electrode and a second electrode in a separated state, and a barrier having electrical insulating properties with a predetermined pattern is provided on the organic layer, to separate the organic electroluminescent devices from each other by the barrier.

This application is a division of prior application Ser. No. 09/211,041filed Dec. 15, 1998, now U.S. Pat. No. 6,232,713.

BACKGROUND OF THE INVENTION

1. Field of the Invention

The present invention relates generally to an organic electroluminescentapparatus having a plurality of organic electroluminescent devices eachhaving an organic layer having luminescent properties provided between ahole injection electrode and an electron injection electrode in aseparated state and a method of fabricating the same, which ischaracterized in that the plurality organic electroluminescent deviceseach having the organic layer having luminescent properties providedbetween the hole injection electrode and the electron injectionelectrode are simply and suitably arranged in a separated state, andparticularly the plurality of organic electroluminescent devices can besuitably separated from each other even when the organic layer havingluminescent properties contains a macromolecular material.

2. Description of the Related Art

In recent years, the needs of flat panel display devices the consumedpower and the size of which are smaller than those of a CRT (cathode-rayTube) which has been heretofore generally employed have been increasedas information equipments are diversified, for example. Anelectroluminescent device has been paid attention to as one of the flatpanel display devices.

The electroluminescent device is roughly divided into an inorganicelectroluminescent device and an organic electroluminescent devicedepending on a used material.

The inorganic electroluminescent device is so adapted that a highelectric field is generally exerted on a luminance portion, andelectrons are accelerated within the high electric field to collide witha luminescence center, whereby the luminescence center is excited toemit light.

On the other hand, the organic electroluminescent device is so adaptedthat electrons and holes are respectively injected into a luminescentportion from an electron injection electrode and a hole injectionelectrode, the electrons and the holes thus injected are recombined witheach other in a luminescence center to bring an organic molecule intoits excited state, and the organic molecule emits fluorescence when itis returned from the excited state to its ground state.

In the case of the inorganic electroluminescent device, a high voltageof 100 to 200 volts is required as its driving voltage because a highelectric field is exerted as described above. On the other hand, theorganic electroluminescent derive can be driven at a low voltage ofapproximately 5 to 20 volts.

In the case of the organic electroluminescent device, a light emittingdevice emitting light in a suitable color can be obtained by selecting afluorescent material that is a luminescent material. It is expected thatthe organic electroluminescent device can be also utilized as amulti-color or full-color display device, for example.

In recent years, fabricated as an organic electroluminescent apparatussuch as an organic electroluminescent panel has been one having aplurality of organic electroluminescent devices, described above,arranged thereon in a separated state.

Conventionally in fabricating the organic electroluminescent apparatushaving the plurality of organic electroluminescent devices arrangedthereon in a separated state, a hole injection electrode has beengenerally formed in a predetermined pattern on a transparent substratesuch as a glass substrate and separated, and an organic layer and anelectron injection electrode which are formed on the hole injectionelectrode have been also respectively formed in predetermined patternsand separated.

Although an operation for forming the hole injection electrode formed ina predetermined pattern on the transparent substrate and separating it,as described above, particularly presents no problem, an operation forrespectively forming the organic layer and the electron injectionelectrode in predetermined patterns on the hole injection electrode andseparating them presents a problem.

Specifically, the organic layer used for the organic electroluminescentdevice is generally low in heat resistance, solvent resistance, andhumidity resistance. When the organic layer and the electron injectionelectrode formed on the organic layer are formed in predeterminedpatterns by photolithography or the like, there are some problems. Forexample, a solvent in photoresist enters the organic layer, the organiclayer is dissolved in an etchant, and an organic layer is damaged byplasma at the time of dry etching.

Therefore, the organic layer and the electron injection electrode havebeen heretofore generally formed in predetermined patterns byevaporation using a mask member. When they are thus evaporated using themask member, however, fine processing cannot be performed.

In recent years, an organic electroluminescent apparatus so adapted thata hole injection electrode is formed in a suitable pattern on atransparent substrate, a barrier having electrical insulating propertieswith a suitable pattern is provided on the transparent substrate, anorganic layer and an electron injection electrode are successivelylaminated by evaporation from above the barrier, and the organic layerand the electron injection electrode are respectively separated by thebarrier has been proposed, as disclosed in JP-A-8-227276, JP-A-8-315981,JP-A-9-102393, etc.

In JP-A-8-315981 and JP-A-9-102393, in providing a patterned barrier 3on a hole injection electrode 2 formed on a transparent substrate 1, anupper surface 3 a of the barrier 3 is increased in size to provide anoverhang portion, as shown in FIG. 1.

When an organic layer 4 is evaporated from above the barrier 3 havingthe overhang portion thus provided by increasing the size of the uppersurface 3 a, the organic layer 4 is not formed under the overhangportion, so that an exposed part of the hole injection electrode 2remains under the overhang portion. When the electron injectionelectrode 5 is then evaporated, the electron injection electrode 5 maybe short-circuited upon being formed on not only the organic layer 4 butalso the exposed part of the hole injection electrode 2.

In recent years, an organic layer having luminescent properties using amacromolecular material that is high in heat stability and is superiorin durability has been paid attention to.

The organic layer containing the macromolecular material can begenerally formed simply by dipping or spin coating. When the patternedbarrier 3 is provided on the hole injection electrode 2 formed on thetransparent substrate 1 as described above, however, the barrier 3interferes with the formation. Therefore, it is difficult to form theorganic layer 4 using the macromolecular material by the above-mentionedmethod.

In the case of the above-mentioned organic layer containing themacromolecular material, erosion by an etchant or the like isrestrained. Consequently, it is considered that an electron injectionelectrode is provided on the organic layer containing the macromolecularmaterial, and the electron injection electrode is formed in apredetermined pattern by photolithography or the like.

When the electron injection electrode is formed in a predeterminedpattern by photolithography or the like, however, it is difficult tocontrol etching because the thickness of the electron injectionelectrode is generally small. Therefore, the etchant penetrates into aportion between the organic layer containing the macromolecular materialand the electron injection electrode, so that some problems occur. Forexample, contact characteristics between the organic layer and theelectron injection electrode are degraded. When an electrode materialhaving a small work function such as magnesium is used as a materialcomposing the electron injection electrode such that electrons areefficiently injected into the organic layer from the electron injectionelectrode, some problems occur. For example, the electron injectionelectrode is degraded upon being oxidized by water or the like of theetchant, so that light cannot be stably emitted.

SUMMARY OF THE INVENTION

An object of the present invention is to make it possible to arrange, inan organic electroluminescent apparatus in which a plurality of organicelectroluminescent devices each having an organic layer havingluminescent properties provided between a hole injection electrode andan electron injection electrode are arranged with they being separatedfrom one another, the electroluminescent devices in a separated statesimply and suitably.

Another object of the present invention is to make it possible to simplyform, when an organic layer having luminescent properties contains amacromolecular material, the organic layer containing the macromolecularmaterial using dipping or spin coating as well as make it possible toarrange organic electroluminescent devices in a separated state simplyand suitably.

In an organic electroluminescent apparatus according to the presentinvention, in arranging a plurality of organic electroluminescentdevices each having an organic layer having luminescent propertiesprovided between a first electrode and a second electrode in a separatedstate, a barrier having electrical insulating properties is formed in apredetermined pattern on the organic layer, to separate the organicelectroluminescent devices from each other by the barrier.

An example of such an organic electroluminescent apparatus is onecomprising a first electrode formed in a predetermined pattern on asubstrate, an organic layer having luminescent properties provided onthe first electrode, a barrier having electrical insulating propertiesformed in a predetermined pattern on the organic layer, and a secondelectrode formed on the organic layer upon being separated by thebarrier having electrical insulating properties.

A method of fabricating an organic electroluminescent apparatusaccording to the present invention comprises the steps of providing afirst electrode in a predetermined pattern on a substrate, providing anorganic layer having luminescent properties on the first electrode,providing a barrier having electrical insulating properties with apredetermined pattern on the organic layer, and providing a secondelectrode separated by the barrier having electrical insulatingproperties on the organic layer.

In the method of fabricating the organic electroluminescent apparatusaccording to the present invention, the first electrode with apredetermined pattern is formed on the substrate, the organic layerhaving luminescent properties is provided on the substrate having thefirst electrode formed thereon, the barrier having electrical insulatingproperties with a predetermined pattern is provided on the organiclayer, and the electron injection electrode is provided from above thebarrier having electrical insulating properties. Consequently, theelectron injection electrode is separated by the barrier, so that theorganic electroluminescent devices are arranged in a separated state.

In the present invention, the barrier having electrical insulatingproperties is provided on the organic layer. Even when the upper surfaceof the barrier is increased in size to provide an overhang portion, thefirst electrode is not exposed under the overhang portion. When thesecond electrode is formed, the second electrode and the first electrodeare not short-circuited upon being brought into contact with each other.

In the present invention, the organic layer is formed, and the barrieris then provided on the organic layer. When the organic layer is formedby painting the substrate having the first electrode formed thereon witha macromolecular material solution by the method of dipping or spincoating, therefore, the barrier does not interfere with the formation.

Examples of the macromolecular material used for the organic layerinclude macromolecular materials having fluorescent properties such as apoly(p-phenylene vinylene) derivative, polythiophene, and polyvinylcarbazole, and macromolecular materials having electrical insulatingproperties, in which a pigment is doped, such as polymethyl methacrylateand polycarbonate.

In providing the barrier having electrically insulating properties onthe organic layer, when a macromolecular material solution for barrierformation is applied, the applied macromolecular material solution forbarrier formation is solidified, and the barrier having electricallyinsulating properties with a predetermined pattern is then formed byetching, used as the macromolecular material in the organic layer is onewhich is insoluble in the macromolecular material solution for barrierformation or an etchant.

Furthermore, in the present invention, when the barrier havingelectrical insulation properties with a predetermined pattern isprovided on the organic layer, and an electrode material is evaporatedfrom above the barrier having electrical insulating properties, toprovide a second electrode on the organic layer separated by the barrierhaving electrical insulating properties, the second electrode formed onthe organic layer need not be formed in a predetermined pattern uponbeing processed by an etchant. Therefore, the possibilities that theetchant penetrates into a portion between the organic layer and thesecond electrode as in the conventional example, so that contactproperties between the organic layer and the second electrode aredegraded, and the second electrode is degraded upon being oxidized areeliminated, so that light can be stably emitted in each of the organicelectroluminescent devices.

There and other objects, advantages and features of the invention willbecome apparent from the following description thereof taken inconjunction with the accompanying drawings which illustrate specificembodiment of the invention.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a partial explanatory view of a conventional organicelectroluminescent device;

FIG. 2 is a plan view showing a state where a plurality of columns ofhole injection electrodes are provided with required spacing on atransparent substrate in an embodiment 1 of the present invention;

FIG. 3 is a schematic explanatory view showing the steps of fabricatingthe organic electroluminescent apparatus in the embodiment 1;

FIG. 4 is a plan view showing a state where a plurality of rows ofbarriers each having an overhang portion are provided on an organiclayer so as to be perpendicular to hole injection electrodes in theembodiment 1; and

FIG. 5 is a schematic explanatory view showing the steps of fabricatingan organic electroluminescent apparatus in an embodiment 4 of thepresent invention.

DESCRIPTION OF THE PREFERRED EMBODIMENTS

An organic electroluminescent apparatus according to an embodiment ofthe present invention and a method of fabricating the same will bespecifically described on the basis of the accompanying drawings.

(Embodiment 1)

In the present embodiment 1, a plurality of columns of transparent holeinjection electrodes 12 each composed of an indium-tin oxide (ITO) wereprovided with required spacing using a normal resist process on atransparent substrate 11 composed of glass, as shown in FIGS. 2 and 3(A).

A hole transporting material composed ofN,N′-diphenyl-N′N-bis(3-methylphenyl)-1,1-biphenyl-4,4′-diamine (TPD)indicated by the following chemical formula 1, a luminescent materialcomposed of a bis(10-hydroxybenzo[h]quinolinate)beryllium complex(BeBq₂) indicated by the following chemical formula 2, and polymethylmethacrylate indicated by the following chemical formula 3 weredissolved in dichloromethane. A solution thus obtained was applied ontothe transparent substrate 11 having the plurality of columns of holeinjection electrodes 12 formed thereon as described above using spincoating, and was then solidified upon being heated at a temperature of120° C., to form an organic layer 13 using a macromolecular material onthe transparent substrate 11 having the hole injection electrodes 12formed thereon.

Positive resist 14′ (Tokyo Ohka Kogyo K. K.: OFPR-1000) was applied soas to have a thickness of 1.5 μm, as shown in FIG. 3 (C), to the organiclayer 13 containing a macromolecular material as described above, washeat-treated, and was then exposed in a predetermined pattern using aphotomask 20, as shown in FIG. 3 (D), in accordance with normalphotolithography in the positive resist 14′. Thereafter, etching wasmade in such a manner that a part, which has not been exposed, of thepositive resist 14′ would remain, to provide a plurality of rows ofbarriers 14 each having an overhang portion provided by increasing thesize of its upper surface 14 a on the organic layer 13 so as to beperpendicular to the hole injection electrodes 12, as shown in FIGS.3(E) and 4.

An electron injection electrode 15 composed of an Al—Li alloy was formedby vacuum evaporation, as shown in FIG. 3(F), on the organic layer 13having the plurality of rows of barriers 14 thus provided thereon, andthe electron injection electrode 15 was separated by the barriers 14, toobtain an organic electroluminescent apparatus having s plurality oforganic electroluminescent devices 10 arranged thereon in a matrix.

In the organic electroluminescent apparatus according to the embodiment1, consider a case where a voltage is applied between the hole injectionelectrodes 12 and the electron injection electrodes 15. In this case,when the voltage was 17 volts, green light having luminance of 1000cd/cm² could be emitted from each of the organic electroluminescentdevices 10. Further, the organic electroluminescent devices 10 weresuitably separated from each other, so that no short also occurred.

(Embodiment 2)

In the present embodiment 2, a plurality of columns of transparent holeinjection electrodes 12 each composed of ITO were provided with requiredspacing on a transparent substrate 11 composed of glass, after whichpoly(p-phenylene vinylene) (PPV) was formed as an organic layer 13 usinga macromolecular material. The organic layer 13 composed of PPV wasformed in accordance with a method described in a document [J. H.Burroughes, et al, Nature, Vol. 347, pp. 539-541 (1990)].

After the organic layer 13 composed of PPV was thus formed, a pluralityof rows of barriers 14 each having an overhang portion by increasing thesize of its upper surface 14 a were provided on the organic layer 13 soas to be perpendicular to the hole injection electrodes 12, an electroninjection electrode 15 composed of an Al—Li alloy was formed on theorganic layer 13 having the barriers 14 thus provided thereon by vacuumevaporation, and the electron injection electrode 15 was separated bythe barriers 14, to obtain an organic electroluminescent apparatushaving a plurality of organic electroluminescent devices 10 arrangedthereon in a matrix. The organic layer 13 composed of PPV was notdissolved in a solution of the above-mentioned positive resist 14′(produced by Tokyo Ohka Kogyo K. K.: OFPR—1000) or an etchant.

In the organic electroluminescent apparatus according to the embodiment2, consider a case where a voltage is applied between the hole injectionelectrodes 12 and the electron injection electrodes 15. In this case,when the voltage was 15 volts, yellow green light having luminance of100 cd/m² could be emitted from each of the organic electroluminescentdevices 10. Further, the organic electroluminescent devices 10 weresuitably separated from each other, so that no short also occurred.

(Embodiment 3)

In the present embodiment 3, an organic electroluminescent apparatus wasfabricated in the same manner as the organic electroluminescentapparatus according to the above-mentioned embodiment 1 except that inproviding an organic layer 13, polycarbonate was used in place of theabove-mentioned polymethyl methacrylate.

In the organic electroluminescent apparatus according to the embodiment3, consider a case where a voltage is applied between hole injectionelectrodes 12 and electron injection electrodes 15. In this case, whenthe voltage was 15 volts, green light having luminance of 1200 cd/m²could be emitted from each of organic electroluminescent devices 10.Further, the organic electroluminescent devices 10 were suitablyseparated from each other, so that no short also occurred.

(Embodiment 4)

Also in the present embodiment 4, a plurality of columns of transparenthole injection electrodes 12 each composed of ITO were provided withrequired spacing on a transparent substrate 11 composed of glass in thesame manner as that in the above-mentioned embodiment 1, and an organiclayer 13 containing the same macromolecular material as that in theembodiment 1 was provided thereon, as shown in FIGS. 5(A) and 5(B).

In the embodiment 4, in providing a plurality of rows of barriers 14 onthe organic layer 13 so as to be perpendicular to the hole injectionelectrodes 12, negative resist 14″ produced by Nippon Zeon K. K. wasused in place of the above-mentioned positive resist 14′ (produced byTokyo Ohka Kogyo K. K.: OFPR—1000), as shown in FIG. 5(C). The negativeresist 14″ was exposed in a predetermined pattern using a photomask 20,as shown in FIG. 5(D), in accordance with normal photolithography in thenegative resist 14″. Thereafter, etching was then made in such a mannerthat a part, which has not been exposed, of the negative resist 14″would remain, to provide a plurality of rows of barriers 14 each havingan overhang portion on its upper surface 14 a so as to be perpendicularto the hole injection electrodes 12. Thereafter, the same steps as thosein the embodiment 1 were carried out, to fabricate an organicelectroluminescent apparatus.

When the barriers 14 were provided using the negative resist 14″ as inthe embodiment 4, it was possible to set the height of the barriers 14to 5 μm. The electron injection electrodes 15 could be more reliablyseparated from each other by the barriers 14, so that the organicelectroluminescent devices 10 could be reliably separated from eachother. Therefore, the yield of the electroluminescent apparatus isimproved by approximately 30%.

Although in each of the above-mentioned embodiments, the transparenthole injection electrodes composed of ITO are provided on thetransparent substrate, the transparent hole injection electrodescomposed of ITO can be also provided on the organic layer after beingseparated from each other by barriers.

Although the present invention has been fully described by way ofexamples, it is to be noted that various changes and modification willbe apparent to those skilled in the art.

Therefore, unless otherwise such changes and modifications depart fromthe scope of the present invention, they should be construed as beingincluded therein.

What is claimed is:
 1. A method of fabricating an organicelectroluminescent apparatus, comprising the steps of: providing a firstelectrode in a predetermined pattern on a substrate; providing anorganic layer having luminescent properties on the first electrode;providing a barrier having electrical insulating properties with apredetermined pattern on the organic layer; and providing a secondelectrode separated by the barrier having electrical insulatingproperties on said organic layer.
 2. The method according to claim 1,wherein the first electrode with a predetermined pattern and the barrierhaving electrical insulating properties with a predetermined pattern areprovided so as to cross each other.
 3. The method according to claim 1,wherein the organic layer having luminescent properties contains amacromolecular material.
 4. The method according to claim 1, wherein theorganic layer is formed by applying a macromolecular material solutionto the substrate having the first electrode formed thereon andsubjecting the solution to annealing processing.
 5. The method accordingto claim 4, wherein a method of applying the macromolecular materialsolution to the substrate having the first electrode formed thereon isspin coating or dipping.
 6. The method according to claim 4, wherein amacromolecular material solution for barrier formation is applied to theorganic layer formed by the annealing processing, and the solution issubjected to annealing processing, to form a barrier having electricalinsulating properties with a predetermined pattern.
 7. The methodaccording to claim 6, wherein the macromolecular material composing saidorganic layer is dissolved in the macromolecular material solution forbarrier formation.
 8. The method according to claim 1, wherein thebarrier having electrical insulating properties with a predeterminedpattern is provided on the organic layer by photolithography.
 9. Themethod according to claim 1, wherein an electrode material is evaporatedfrom above the barrier having electrical insulating properties, toprovide a second electrode separated by the barrier having electricalinsulating properties on the organic layer.
 10. The method according toclaim 1, wherein said barrier having electrical insulating propertiescontains a macromolecular material.
 11. The method according to claim10, wherein the macromolecular material composing said barrier is aresist material.